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1.
Nat Commun ; 15(1): 3828, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38714653

RESUMO

Stabilization of topological spin textures in layered magnets has the potential to drive the development of advanced low-dimensional spintronics devices. However, achieving reliable and flexible manipulation of the topological spin textures beyond skyrmion in a two-dimensional magnet system remains challenging. Here, we demonstrate the introduction of magnetic iron atoms between the van der Waals gap of a layered magnet, Fe3GaTe2, to modify local anisotropic magnetic interactions. Consequently, we present direct observations of the order-disorder skyrmion lattices transition. In addition, non-trivial topological solitons, such as skyrmioniums and skyrmion bags, are realized at room temperature. Our work highlights the influence of random spin control of non-trivial topological spin textures.

2.
ACS Appl Mater Interfaces ; 16(19): 25432-25444, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38688003

RESUMO

Encapsulating an electrocatalytic material with a semipermeable, nanoscopic oxide overlayer offers a promising approach to enhancing its stability, activity, and/or selectivity compared to an unencapsulated electrocatalyst. However, applying nanoscopic oxide encapsulation layers to high-surface-area electrodes such as nanoparticle-supported porous electrodes is a challenging task. This study demonstrates that the recently developed condensed layer deposition (CLD) method can be used for depositing nanoscopic (sub-10 nm thick) titanium dioxide (TiO2) overlayers onto high-surface-area platinized carbon foam electrodes. Characterization of the overlayers by transmission electron microscopy (TEM) and electron energy loss spectroscopy (EELS) showed that the films are amorphous, while X-ray photoelectron spectroscopy confirmed that they exhibit TiO2 stoichiometry. Electrodes were also characterized by hydrogen underpotential deposition (Hupd) and carbon monoxide (CO) stripping, demonstrating that the Pt electrocatalysts remain electrochemically active after encapsulation. Additionally, copper underpotential deposition (Cuupd) measurements revealed that TiO2 overlayers are effective at blocking Cu2+ from reaching the TiO2/Pt buried interface and were used to estimate that between 43 and 98% of Pt surface sites were encapsulated. Overall, this study shows that CLD is a promising approach for depositing nanoscopic protective overlayers on high-surface-area electrodes.

3.
J Gen Virol ; 105(1)2024 01.
Artigo em Inglês | MEDLINE | ID: mdl-38271027

RESUMO

The COVID-19 pandemic has highlighted the need for vaccines capable of providing rapid and robust protection. One way to improve vaccine efficacy is delivery via microarray patches, such as the Vaxxas high-density microarray patch (HD-MAP). We have previously demonstrated that delivery of a SARS-CoV-2 protein vaccine candidate, HexaPro, via the HD-MAP induces potent humoral immune responses. Here, we investigate the cellular responses induced by HexaPro HD-MAP vaccination. We found that delivery via the HD-MAP induces a type one biassed cellular response of much greater magnitude as compared to standard intramuscular immunization.


Assuntos
COVID-19 , Glicoproteína da Espícula de Coronavírus , Animais , Camundongos , Humanos , Glicoproteína da Espícula de Coronavírus/genética , Pandemias , COVID-19/prevenção & controle , SARS-CoV-2 , Vacinação , Imunidade Celular , Vacinas contra COVID-19 , Anticorpos Antivirais , Imunidade Humoral , Anticorpos Neutralizantes
4.
Adv Mater ; 36(13): e2305739, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37800466

RESUMO

Magnetic van der Waals heterostructures provide a unique platform to study magnetism and spintronics device concepts in the 2D limit. Here, studies of exchange bias from the van der Waals antiferromagnet CrSBr acting on the van der Waals ferromagnet Fe3GeTe2 (FGT) are reported. The orientation of the exchange bias is along the in-plane easy axis of CrSBr, perpendicular to the out-of-plane anisotropy of the FGT, inducing a strongly tilted magnetic configuration in the FGT. Furthermore, the in-plane exchange bias provides sufficient symmetry breaking to allow deterministic spin-orbit torque switching of the FGT in CrSBr/FGT/Pt samples at zero applied magnetic field. A minimum thickness of the CrSBr of >10 nm is needed to provide a non-zero exchange bias at 30 K.

5.
Adv Mater ; 36(9): e2308555, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38016700

RESUMO

2D layered materials with broken inversion symmetry are being extensively pursued as  spin source layers to realize high-efficiency magnetic switching. Such low-symmetry layered systems are, however, scarce. In addition, most layered magnets with perpendicular magnetic anisotropy show a low Curie temperature. Here, the experimental observation of spin-orbit torque magnetization self-switching at room temperature in a layered polar ferromagnetic metal, Fe2.5 Co2.5 GeTe2 is reported. The spin-orbit torque is generated from the broken inversion symmetry along the c-axis of the crystal. These results provide a direct pathway toward applicable 2D spintronic devices.

6.
Sci Adv ; 9(50): eadi4540, 2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-38091392

RESUMO

We present measurements of thermally generated transverse spin currents in the topological insulator Bi2Se3, thereby completing measurements of interconversions among the full triad of thermal gradients, charge currents, and spin currents. We accomplish this by comparing the spin Nernst magneto-thermopower to the spin Hall magnetoresistance for bilayers of Bi2Se3/CoFeB. We find that Bi2Se3 does generate substantial thermally driven spin currents. A lower bound for the ratio of spin current density to thermal gradient is [Formula: see text] = (4.9 ± 0.9) × 106 [Formula: see text], and a lower bound for the magnitude of the spin Nernst ratio is -0.61 ± 0.11. The spin Nernst ratio for Bi2Se3 is the largest among all materials measured to date, two to three times larger compared to previous measurements for the heavy metals Pt and W. Strong thermally generated spin currents in Bi2Se3 can be understood via Mott relations to be due to an overall large spin Hall conductivity and its dependence on electron energy.

7.
Clin Transl Immunology ; 12(12): e1476, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-38050635

RESUMO

Objective: Class III obesity (body mass index [BMI] ≥ 40 kg m-2) significantly impairs the immune response to SARS-CoV-2 vaccination. However, the effect of an elevated BMI (≥ 25 kg m-2) on humoral immunity to SARS-CoV-2 infection and COVID-19 vaccination remains unclear. Methods: We collected blood samples from people who recovered from SARS-CoV-2 infection approximately 3 and 13 months of post-infection (noting that these individuals were not exposed to SARS-CoV-2 or vaccinated in the interim). We also collected blood samples from people approximately 5 months of post-second dose COVID-19 vaccination (the majority of whom did not have a prior SARS-CoV-2 infection). We measured their humoral responses to SARS-CoV-2, grouping individuals based on a BMI greater or less than 25 kg m-2. Results: Here, we show that an increased BMI (≥ 25 kg m-2), when accounting for age and sex differences, is associated with reduced antibody responses after SARS-CoV-2 infection. At 3 months of post-infection, an elevated BMI was associated with reduced antibody titres. At 13 months of post-infection, an elevated BMI was associated with reduced antibody avidity and a reduced percentage of spike-positive B cells. In contrast, no significant association was noted between a BMI ≥ 25 kg m-2 and humoral immunity to SARS-CoV-2 at 5 months of post-secondary vaccination. Conclusions: Taken together, these data showed that elevated BMI is associated with an impaired humoral immune response to SARS-CoV-2 infection. The impairment of infection-induced immunity in individuals with a BMI ≥ 25 kg m-2 suggests an added impetus for vaccination rather than relying on infection-induced immunity.

8.
Mol Ther Nucleic Acids ; 34: 102056, 2023 Dec 12.
Artigo em Inglês | MEDLINE | ID: mdl-38028199

RESUMO

Zika virus (ZIKV) infections are spreading silently with limited global surveillance in at least 89 countries and territories. There is a pressing need to develop an effective vaccine suitable for equitable distribution globally. Consequently, we previously developed a proprietary DNA vaccine encoding secreted non-structural protein 1 of ZIKV (pVAX-tpaNS1) to elicit rapid protection in a T cell-dependent manner in mice. In the current study, we evaluated the stability, efficacy, and immunogenicity of delivering this DNA vaccine into the skin using a clinically effective and proprietary high-density microarray patch (HD-MAP). Dry-coating of pVAX-tpaNS1 on the HD-MAP device resulted in no loss of vaccine stability at 40°C storage over the course of 28 days. Vaccination of mice (BALB/c) with the HD-MAP-coated pVAX-tpaNS1 elicited a robust anti-NS1 IgG response in both the cervicovaginal mucosa and systemically and afforded protection against live ZIKV challenge. Furthermore, the vaccination elicited a significantly higher magnitude and broader NS1-specific T helper and cytotoxic T cell response in vivo compared with traditional needle and syringe intradermal vaccination. Overall, the study highlights distinctive immunological advantages coupled with an excellent thermostability profile of using the HD-MAP device to deliver a novel ZIKV DNA vaccine.

9.
Vaccines (Basel) ; 11(11)2023 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-38006057

RESUMO

Microarray patches (MAPs) have the potential to be a safer, more acceptable, easier-to-use, and more cost-effective means for the administration of vaccines than injection by needle and syringe. Here, we report findings from a randomized, partially double-blinded, placebo-controlled Phase I trial using the Vaxxas high-density MAP (HD-MAP) to deliver a measles rubella (MR) vaccine. Healthy adults (N = 63, age 18-50 years) were randomly assigned 1:1:1:1 to four groups: uncoated (placebo) HD-MAPs, low-dose MR HD-MAPs (~3100 median cell-culture infectious dose [CCID50] measles, ~4300 CCID50 rubella); high-dose MR-HD-MAPs (~9300 CCID50 measles, ~12,900 CCID50 rubella); or a sub-cutaneous (SC) injection of an approved MR vaccine, MR-Vac (≥1000 CCID50 per virus). The MR vaccines were stable and remained viable on HD-MAPs when stored at 2-8 °C for at least 24 months. When MR HD-MAPs stored at 2-8 °C for 24 months were transferred to 40 °C for 3 days in a controlled temperature excursion, loss of potency was minimal, and MR HD-MAPs still met World Health Organisation (WHO) specifications. MR HD-MAP vaccination was safe and well-tolerated; any systemic or local adverse events (AEs) were mild or moderate. Similar levels of binding and neutralizing antibodies to measles and rubella were induced by low-dose and high-dose MR HD-MAPs and MR-Vac. The neutralizing antibody seroconversion rates on day 28 after vaccination for the low-dose HD-MAP, high-dose HD-MAP and MR-Vac groups were 37.5%, 18.8% and 35.7%, respectively, for measles, and 37.5%, 25.0% and 35.7%, respectively, for rubella. Most participants were seropositive for measles and rubella antibodies at baseline, which appeared to negatively impact the number of participants that seroconverted to vaccines delivered by either route. The data reported here suggest HD-MAPs could be a valuable means for delivering MR-vaccine to hard-to-reach populations and support further development. Clinical trial registry number: ACTRN12621000820808.

10.
Chem Sci ; 14(43): 12345-12354, 2023 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-37969574

RESUMO

A mixture of N,N,N'-trisubstituted thiourea and cyclic N,N,N',N'-tetrasubstituted selenourea precursors were used to synthesize three monolayer thick CdS1-xSex nanoplatelets in a single synthetic step. The microstructure of the nanoplatelets could be tuned from homogeneous alloys, to graded alloys to core/crown heterostructures depending on the relative conversion reactivity of the sulfur and selenium precursors. UV-visible absorption and photoluminescence spectroscopy and scanning transmission electron microscopy electron energy loss spectroscopy (STEM-EELS) images demonstrate that the elemental distribution is governed by the relative precursor conversion kinetics. Slow conversion kinetics produced nanoplatelets with larger lateral dimensions, behavior that is characteristic of precursor conversion limited growth kinetics. Across a 10-fold range of reactivity, CdS nanoplatelets have 4× smaller lateral dimensions than CdSe nanoplatelets grown under identical conversion kinetics. The difference in size is consistent with a rate of CdSe growth that is 4× greater than the rate of CdS. The influence of the relative sulfide and selenide growth rates, the duration of the nucleation phase, and the solute composition on the nanoplatelet microstructure are discussed.

11.
Expert Rev Vaccines ; 22(1): 937-955, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37846657

RESUMO

INTRODUCTION: Microneedles are emerging as a promising technology for vaccine delivery, with numerous advantages over traditional needle and syringe methods. Preclinical studies have demonstrated the effectiveness of MAPs in inducing robust immune responses over traditional needle and syringe methods, with extensive studies using vaccines targeted against different pathogens in various animal models. Critically, the clinical trials have demonstrated safety, immunogenicity, and patient acceptance for MAP-based vaccines against influenza, measles, rubella, and SARS-CoV-2. AREAS COVERED: This review provides a comprehensive overview of the different types of microarray patches (MAPs) and analyses of their applications in preclinical and clinical vaccine delivery settings. This review also covers additional considerations for microneedle-based vaccination, including adjuvants that are compatible with MAPs, patient safety and factors for global vaccination campaigns. EXPERT OPINION: MAP vaccine delivery can potentially be a game-changer for vaccine distribution and coverage in both high-income and low- and middle-income countries. For MAPs to reach this full potential, many critical hurdles must be overcome, such as large-scale production, regulatory compliance, and adoption by global health authorities. However, given the considerable strides made in recent years by MAP developers, it may be possible to see the first MAP-based vaccines in use within the next 5 years.


Assuntos
Vacinas contra Influenza , Influenza Humana , Sarampo , Rubéola (Sarampo Alemão) , Animais , Humanos , Rubéola (Sarampo Alemão)/prevenção & controle , Vacinação/métodos , Sarampo/prevenção & controle , Agulhas
12.
J Am Chem Soc ; 145(31): 17406-17419, 2023 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-37525439

RESUMO

While certain ternary spinel oxides have been well-explored with colloidal nanochemistry, notably the ferrite spinel family, ternary manganese (Mn)-based spinel oxides have not been tamed. A key composition is cobalt (Co)-Mn oxide (CMO) spinel, CoxMn3-xO4, that, despite exemplary performance in multiple electrochemical applications, has few reports in the colloidal literature. Of these reports, most show aggregated and polydisperse products. Here, we describe a synthetic method for small, colloidally stable CMO spinel nanocrystals with tunable composition and low dispersity. By reacting 2+ metal-acetylacetonate (M(acac)2) precursors in an amine solvent under an oxidizing environment, we developed a pathway that avoids the highly reducing conditions of typical colloidal synthesis reactions; these reducing conditions typically push the system toward a monoxide impurity phase. Through surface chemistry studies, we identify organic byproducts and their formation mechanism, enabling us to engineer the surface and obtain colloidally stable nanocrystals with low organic loading. We report a CMO/carbon composite with low organic contents that performs the oxygen reduction reaction (ORR) with a half-wave potential (E1/2) of 0.87 V vs RHE in 1.0 M potassium hydroxide at 1600 rpm, rivaling previous reports for the highest activity of this material in ORR electrocatalysis. We extend the general applicability of this procedure to other Mn-based spinel nanocrystals such as Zn-Mn-O, Fe-Mn-O, Ni-Mn-O, and Cu-Mn-O. Finally, we show the scalability of this method by producing inorganic nanocrystals at the gram scale.

13.
Microsc Microanal ; 29(Supplement_1): 2104, 2023 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-37612962
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